Sluggish redox kinetics and severe polysulfide shuttling are major hurdles for the commercialization of lithium–sulfur (Li–S) batteries. Transition‐metal compound catalysts offer a promising solution by providing excellent polysulfide adsorption capabilities, outstanding catalytic activities, and homogeneous nucleation control of Li2S2/Li2S. The electronic structure of transition‐metal sites in catalysts can also be fine‐tuned through bi‐metallic coupling, which can further improve the catalytic activities. In this study, bi‐metallic nickel molybdenum phosphide is co‐synthesized with Li2S and carbon through a carbothermal reduction process, forming a cathode composite (Li2S @ NixMoyPz @ C). This process is not only advantageous for large‐scale manufacturing due to its simplicity, but also ensures homogeneous integration and distribution of the catalyst within the cathode composite. Furthermore, applying Li2S as an active material allows the creation of an anode‐free cell configuration, enhancing the overall cell energy density. The anode‐free cell with the Li2S @ NixMoyPz @ C composite cathode demonstrates an outstanding capacity retention of 50% over 300 cycles at a negative‐to‐positive capacity (N/P) ratio of 1. Additionally, the bi‐metallic phosphide integrated Li2S cathode composite delivers a remarkable anode‐free pouch cell performance of 703 mA h g−1 (on Li2S basis) under the challenging conditions of an E/Li2S ratio of 4.5.

中文翻译：

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用于高性能无阳极锂硫电池的双金属磷化物电催化剂集成Li2S正极


缓慢的氧化还原动力学和严重的多硫化物穿梭是锂硫（Li-S）电池商业化的主要障碍。过渡金属化合物催化剂通过提供优异的多硫化物吸附能力、出色的催化活性和Li2S2/Li2S的均相成核控制，提供了一种有前途的解决方案。催化剂中过渡金属位点的电子结构也可以通过双金属耦合进行微调，从而进一步提高催化活性。在这项研究中，双金属镍钼磷化物通过碳热还原过程与Li2S和碳共合成，形成阴极复合材料（Li2S@NixMoyPz@C）。该工艺不仅由于其简单性而有利于大规模制造，而且还确保了催化剂在阴极复合材料内的均匀集成和分布。此外，应用Li2S作为活性材料可以创建无阳极电池配置，从而提高电池的整体能量密度。采用 Li2S @ NixMoyPz @ C 复合阴极的无阳极电池在负正容量 (N/P) 比为 1 的情况下，在 300 次循环中表现出 50% 的出色容量保持率。此外，集成的双金属磷化物Li2S 阴极复合材料在 E/Li2S 比为 4.5 的挑战性条件下提供了 703 mA h g−1 的卓越无阳极软包电池性能（以 Li2S 为基础）。